We experimentally investigated conductivity and mobility of poly(3-hexylthiophene) (P3HT) doped with tetrafluorotetracyanoquinodimethane (F 4 TCNQ) for various relative doping concentrations ranging from ultralow (10 −5 ) to high (10 −1 ) and various active layer thicknesses. Although the measured conductivity monotonously increases with increasing doping concentration, the mobilities decrease, in agreement with previously published work. Additionally, we developed a simple yet quantitative model to rationalize the results on basis of a modification of the density of states (DOS) by the Coulomb potentials of ionized dopants. The DOS was integrated in a three-dimensional (3D) hopping formalism in which parameters such as energetic disorder, intersite distance, energy level difference, and temperature were varied. We compared predictions of our model as well as those of a previously developed model to kinetic Monte Carlo (MC) modeling and found that only the former model accurately reproduces the mobility of MC modeling in a large part of the parameter space. Importantly, both our model and MC simulations are in good agreement with experiments; the crucial ingredient to both is the formation of a deep trap tail in the Gaussian DOS with increasing doping concentration.
We investigate conductivity and mobility of different hosts mixed with different electron-withdrawing guests in concentrations ranging from ultralow to high. The effect of the guest material on the mobility and conductivity of the host material varies systematically with the guests' LUMO energy relative to the host HOMO, in quantitative agreement with a recently developed model. For guests with a LUMO within ∼0.5 eV of the host HOMO the dominant process governing transport is the competition between the formation of a deep tail in the host DOS and state filling. In other cases, the interaction with the host is dominated by any polar side groups on the guest and changes in the host morphology. For relatively amorphous hosts the latter interaction can lead to a suppression of deep traps, causing a surprising mobility increase by 1−2 orders of magnitude. In order to analyze our data, we developed a simple method to diagnose both the presence and the filling of traps.
The recent upswing in attention for the thermoelectric properties of organic semiconductors (OSCs) adds urgency to the need for a quantitative description of the range and energetics of hopping transport in organic semiconductors under relevant circumstances, i.e., around room temperature (RT). In particular, the degree to which hops beyond the nearest neighbor must be accounted for at RT is still largely unknown. Here, measurements of charge and energy transport in doped OSCs are combined with analytical modeling to reach the univocal conclusion that variable-range hopping is the proper description in a large class of disordered OSC at RT. To obtain quantitative agreement with experiment, one needs to account for the modification of the density of states by ionized dopants. These Coulomb interactions give rise to a deep tail of trap states that is independent of the material's initial energetic disorder. Insertion of this effect into a classical Mott-type variable-range hopping model allows one to give a quantitative description of temperature-dependent conductivity and thermopower measurements on a wide range of disordered OSCs. In particular, the model explains the commonly observed quasiuniversal power-law relation between the Seebeck coefficient and the conductivity.
A major attraction of organic conjugated semiconductors is that materials with new, emergent functionality can be designed and made by simple blending, as is extensively used in e.g. bulk heterojunction organic solar cells. Here, we critically review doped blends based on organic semiconductors (OSC) for thermoelectric applications. Several experimental strategies to improve thermoelectric performance, measured in terms of power factor (PF) or figure-ofmerit ZT, have been demonstrated in recent literature. Specifically, density-of-states design in blends of 2 OSCs can be used to obtain electronic Seebeck coefficients up to ∼2000 µV/K. Alternatively, blending with (high-dielectric constant) insulating polymers can improve doping efficiency and thereby conductivity, as well as induce more favorable morphologies that improve conductivity while hardly affecting thermopower. In the PEDOT:PSS blend system, processing schemes to either improve conductivity via morphology or via (partial) removal of the electronically isolating PSS, or both, have been demonstrated. Although a range of experiments have at least quasi-quantitatively been explained by analytical or numerical models, a comprehensive model for organic thermoelectrics is lacking so far.Strategies to increase thermoelectric performance of doped organic semiconductors by blending are reviewed. Experimental results are, where possible, compared to analytical and numerical models. Several promising strategies to increase conductivity and/or thermopower are experimentally identified in recent literature. In contrast, formal understanding, especially of the role of morphology, is somewhat lagging behind.
Recent developments in mobile brain-body imaging (MoBI) technologies have enabled studies of human locomotion where subjects are able to move freely in more ecologically valid scenarios. In this study, MoBI was employed to describe the behavioral and neurophysiological aspects of three different commonly occurring walking conditions in healthy adults. The experimental conditions were self-paced walking, walking while conversing with a friend and lastly walking while texting with a smartphone. We hypothesized that gait performance would decrease with increased cognitive demands and that condition-specific neural activation would involve condition-specific brain areas. Gait kinematics and high density electroencephalography (EEG) were recorded whilst walking around a university campus. Conditions with dual tasks were accompanied by decreased gait performance. Walking while conversing was associated with an increase of theta (θ) and beta (β) neural power in electrodes located over left-frontal and right parietal regions, whereas walking while texting was associated with a decrease of β neural power in a cluster of electrodes over the frontal-premotor and sensorimotor cortices when compared to walking whilst conversing. In conclusion, the behavioral “signatures” of common real-life activities performed outside the laboratory environment were accompanied by differing frequency-specific neural “biomarkers”. The current findings encourage the study of the neural biomarkers of disrupted gait control in neurologically impaired patients.
We investigate the suitability of the “sequential doping” method of organic semiconductors for thermoelectric applications. The method consists of depositing a dopant (F4TCNQ) containing solution on a previously cast semiconductor (P3HT) thin film to achieve high conductivity, while preserving the morphology. For very thin films (∼25 nm), we achieve a high power factor around 8 μW/mK−2 with a conductivity over 500 S/m. For the increasing film thickness, conductivity and power factor show a decreasing trend, which we attribute to the inability to dope the deeper parts of the film. Since thick films are required to extract significant power from thermoelectric generators, we developed a simple additive technique that allows the deposition of an arbitrary number of layers without significant loss in conductivity or power factor that, for 5 subsequent layers, remain at ∼300 S/m and ∼5 μW/mK−2, respectively, whereas the power output increases almost one order of magnitude as compared to a single layer. The efficient doping in multilayers is further confirmed by an increased intensity of (bi)polaronic features in the UV-Vis spectra.
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